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>Magister Scientiae - MSc / It is well known, that there is a severe lack of information available pertaining to neutron rich nuclei, specifically of those nuclei with mass numbers ≥ 60. These neutron rich nuclei are not easy to access in current experimental facilities or be produced with sufficient yield to allow for it to be studied. In order to expand our understanding of nuclear physics by studying the properties and characteristics of these nuclei, the development of new facilities producing Radioactive-ion Beams (RIBs) is required. The applications for RIBs are wide, allowing for deeper investigations into the properties of nuclei, their interactions and the manner in which they were formed in the early universe. Additionally, there are various interdisciplinary fields such as medicine, biology and material science in which RIBs can be utilized as a driving mechanism for new research and technological innovation. The iThemba Laboratory for Accelerator Based Sciences (iThemba LABS), South Africa, has proposed a new facility for the production and acceleration of radioactive-ion beams (RIBs). The RIB Project is to be developed in sequential phases and would produce a range of neutron-rich isotopes for low-energy materials science and nuclear physics research. Of specific interest, is the production of the Helium-6 isotope (6He), for its potential applications in various areas of nuclear physics research. The aim of this research work was to design, model and optimise a RIB production target capable of producing high intensity 6He beams, guided by the characteristics of the primary proton beam available for use at iThemba LABS. This research work/design study is however limited, due to the absence of experimentally measured and verified 6He cross section data for proton induced reactions on the proposed target materials (Graphite and Boron Carbide). However, best-estimate approaches were adopted through the use of validated computer codes. Additionally, all 6He yield results are presented as in-target yields, as this study did not cover the diffusion (isotope release) efficiency of the target systems in question. Three RIB production targets types were investigated using Graphite, Boron Carbide and Beryllium Oxide as potential target materials. Following numerous optimisation processes, a Boron Carbide RIB target was converged upon, proving to be suitable for the production of high intensity 6He beams at iThemba LABS, by meeting the material thermal and mechanical limiting criteria for operation. This target system was found to produce an in-target 6He yield rate of 2 ~ 3 x 1011 6He/s, considered sufficient for experimental application at iThemba LABS.

O campo da modificação de materiais, através da implantação iônica, vem crescendo amplamente, impulsionado pelas aplicações tecnológicas na biologia, medicina, eletrônica, e outras áreas. Um dos aspectos relacionados ao entendimento desses novos materiais é a identificação e caracterização dos danos produzidos, após a irradiação. Nesse trabalho, foi proposto estudar as modificações microscópicas, após irradiação com feixe de íons de alta energia, em três diferentes polímeros: o policarbonato(Makrofol KG), com espessura de 8 µm; o polialil diglicol carbonato PADC (CR39), espessura 900 µm; e o nitrato de celulose (LR115), espessura 12µm. As amostras foram irradiadas com feixe de Au de 350 MeV no acelerador Cíclotron do Hahn-Meitner Institut (HMI) em Berlim. As amostras de Makrofol KG foram dispostas em superposição de 6 folhas posicionadas perpendicularmente à direção do feixe e foram irradiadas com fluências de 10^8, 10^9 e 10^11 íons/cm^2. As amostras de CR39 e LR115 foram irradiadas com fluência de 10^9 íons/cm^2, sem superposição das amostras. O estudo comparativo dos danos estruturais nas amostras, antes e após a irradiação, foi realizado através de técnicas analíticas como Espectroscopia de Absorção no Infravermelho por Transformada de Fourier (FTIR), Difração de Raios X (XRD), Análise com Detecção de Recuo Elástico (ERDA), e Corrosão Química, para visualização e caracterização dos poros através do microscópio óptico e microscópio eletrônico de varredura. A análise FTIR das amostras mostrou haver diminuição do número de ligações simples, em favor do aumento do número de ligações duplas e triplas, após irradiação das amostras. Além disso, observou-se que a intensidade dos danos observados aumenta com o poder de freamento médio dos íons de Au durante a penetração nas amostras. A análise XRD, por sua vez, permitiu verificar um decréscimo da cristalinidade do Makrofol KG irradiado, enquanto observou-se indicações de variação da densidade do CR39, após irradiação, e inexistência de variação no LR115. A metodologia proposta para análise das amostras através da técnica ERDA não se mostrou eficiente para determinar a variação no teor de H das mesmas após a irradiação, não sendo possível obter resultados conclusivos para as amostras. Na análise dos poros, após corrosão química, observou-se diferentes comportamentos. As amostras de CR39 apresentaram uma evolução de superfície porosa para superfície pontiaguda com o aumento do tempo de corrosão, e obteve-se o valor Va = 1,213 (17) µm/h para a velocidade de abertura do poros. Por outro lado, as diferentes folhas de Makrofol KG mantiveram a topografia porosa, sendo que a velocidade de abertura dos poros apresentou dependência com o poder de freamento dos íons na irradiação. Comparando amostras com valores semelhantes do poder de freamento, o resultado de Va obtido para o Makrofol é cerca de três vezes maior que o obtido para o CR39. / The research in the field of material modification with ion implantation has greately improved, stimulated by technological applications in biology, medicine, electronics and other related areas. One of the correlated aspects in understanding these new materials is the identification and characterization of the damage produced by ion beam irradiation. In this work, we propose to identify the microscopic modification in polymers, after their irradiation with a high energy beam. Three polymers have been used: polycarbonate foils (Makrofol KG), 8 µm thick; polyalyl diglycol carbonate PADC (CR39) 900 µm thick and cellulose nitrate(LR115) 12 µm thick. The samples were irradiated with 350 MeV Au beam from the Cyclotron accelerator at Hahn-Meitner Institut (HMI) in Berlin. The Makrofol samples were placed in a 6-foil stack positioned in normal direction relative to the incident beam, in order to stop the projectiles. The irradiations were performed with ion fluences of 10^8, 10^9 e 10^11 ions/cm^2. The CR39 and LR115 samples, thicker than the range, were irradiated with the fluency of 10^9 ions/cm^2. The investigation of structural damage in the samples, after irradiation, was performed through analytical techniques such as: Fourier Transform Infrared Absorption Spectroscopy (FTIR), X Ray Difraction (XRD), Elastic Recoil Detection Analysis (ERDA), and Etching, followed by pore characterization using an optical and a scanning electron microscopes. The FTIR analysis of the samples showed a decrease in the number of simple bonds and an increase in the number of double and triple bonds, after irradiation. Moreover, it was observed that the damage intensity increases with the mean stopping power of Au. The XRD analysis allowed the observation of crystallinity decrease in Makrofol, and gave indications about a possible deviation in CR39 density, after sample irradiation, and no variation in LR115 samples. The methodology proposed using ERDA technique was not eficient to determine the H atoms teor in the polymers after irradiation, so, it was not possible to get conclusive results from the data. In the pore analysis, after etching, different behaviors were observed. The CR39 samples showed an evolution from a porous surface to a sharply peaked surface and a pore opening rate Va = 1,213 (17) µm/h was obtained. On the contrary, different Makrofol KG foils preserved the porous topography for different etching times. The pore opening rate showed dependence with ion stopping power in the irradiation. Comparing samples with similar values of stopping power, the result is that Makrofol Va is three times greater than the obtained to CR39.

Doctor of Philosophy / Department of Physics / Itzhak Ben-Itzhak / The use of ultrafast lasers allows one to study and even control quantum mechanical systems on their natural timescales. Our aim is to study the fragmentation of small molecules in strong laser fields as a means to gain understanding of molecular dynamics and light-matter interactions. Our research group has utilized fast, positively charged molecular ion beams as targets to study and control fragmentation by strong laser fields. This approach allows for detection of all molecular fragments including neutrals, and a coincidence three-dimensional momentum imaging technique is used to characterize the fragmentation. A natural extension of these types of studies is to expand the types of molecular systems that can be studied, from positively charged molecules to neutral and negatively charged molecules. To that end, the primary technical development of this dissertation involved the generation and use of fast, negatively charged molecular beams. Using fast molecular anion beams as targets allows for the study of fragmentation in which all fragments are neutral. As a demonstration, we employ this capability to study F2- dissociation and photodetachment. The dissociation pathways are identified and used to evaluate the initial vibrational population of the F2- beam. The role of dissociation in photodetachment is also explored, and we find that it competes with other dissociative (F+F) and non-dissociative (F2) photodetachment mechanisms. Also highlighted are studies of fragmentation of LiO-, in which the dissociation into Li+O- fragments provides information about the structure of Li O-, including the bond dissociation energy, which was found to be larger than values based on theory. Studies of the autodetachment lifetimes of Li O- were also performed using a pump-probe technique. Additional experimental advancements have made successful pump-probe studies of the ionization of HD+ and Ar2+ possible. Enhancement in the ionization of dissociating HD+ and Ar2+ was observed at surprisingly large internuclear separation where the fragments are expected to behave like separate atoms. The analysis methods used to quantify this enhancement are also described. Finally, the production of excited Rydberg D* fragments from D2 molecules was studied utilizing a state-selective detection method. The carrier-envelope phase dependence of D* formation was found to depend on the range of excited final states of the atomic fragments. We also measured the excited state population of the D* fragments. Together, the studies presented in this work provide new information about fragmentation of positive, negative, and neutral molecules in strong laser fields, and the experimental developments serve as building blocks for future studies that will lead to a better understanding of molecular dynamics.

Plant cell walls compose the largest source of sugars on earth and are a potential source after conversion for liquid transportation fuels. However, the crystalline region of cellulose and the lignin that incases it present significant obstacles for enzymes to digest. This lowers the sugar yield, which ultimately decreases the production efficiency of bioethanol. A pretreatment that could help lowering the amount of crystallinity; meanwhile, breakdown the matrix of lignin and polysaccharides that cover cellulose fibers would be ideal. Here we propose a physical pretreatment strategy of electron beam irradiation that could potentially decrease cellulose crystallinity as well as unzip the lignin structure. Four types of biomass: cellulose, yellow pine, yellow poplar, and switchgrass were irradiated with a 12 MeV electron beam (Sterigenics, Inc.) at dosages of 0, 54, 80, 148 and 403 kGy. By combining the result from the wet chemical analysis of percent weight glucose/ cellulose from the HPLC, percent crystallinity from the Wide Angle X-Ray Diffraction (WAX) and the change of chemical functionality from Fourier Transform Infrared Spectrometer (FTIR), a promising effect is obtained in pine and yellow poplar but not in cellulose and switchgrass. A significant increase in percent glucose is observed for pine at higher doses as shown by (r = 0.97, P< 0.0076) which are 9.4 and 27% at 0 and 403 kGy. The amount of glucose considerably changes from all different types of biomass over time (P< 0.0001). A strong correlation of decreasing in percent crystallinity was found in poplar (r = -0.89, P< 0.05) from 32.4% to 17.4% and related to an average increase in percent glucose produced from 30 to 55% comparing between 0 and 403 kGy.

Plant cell walls compose the largest source of sugars on earth and are a potential source after conversion for liquid transportation fuels. However, the crystalline region of cellulose and the lignin that incases it present significant obstacles for enzymes to digest. This lowers the sugar yield, which ultimately decreases the production efficiency of bioethanol. A pretreatment that could help lowering the amount of crystallinity; meanwhile, breakdown the matrix of lignin and polysaccharides that cover cellulose fibers would be ideal. Here we propose a physical pretreatment strategy of electron beam irradiation that could potentially decrease cellulose crystallinity as well as unzip the lignin structure. Four types of biomass: cellulose, yellow pine, yellow poplar, and switchgrass were irradiated with a 12 MeV electron beam (Sterigenics, Inc.) at dosages of 0, 54, 80, 148 and 403 kGy. By combining the result from the wet chemical analysis of percent weight glucose/ cellulose from the HPLC, percent crystallinity from the Wide Angle X-Ray Diffraction (WAX) and the change of chemical functionality from Fourier Transform Infrared Spectrometer (FTIR), a promising effect is obtained in pine and yellow poplar but not in cellulose and switchgrass. A significant increase in percent glucose is observed for pine at higher doses as shown by (r = 0.97, P< 0.0076) which are 9.4 and 27% at 0 and 403 kGy. The amount of glucose considerably changes from all different types of biomass over time (P< 0.0001). A strong correlation of decreasing in percent crystallinity was found in poplar (r = -0.89, P< 0.05) from 32.4% to 17.4% and related to an average increase in percent glucose produced from 30 to 55% comparing between 0 and 403 kGy.

In this thesis, Gallium Nitride (GaN) micro- and nanostructures were fabricated based on focused ion beam (FIB) milling. The starting wafer is an epitaxial structure containing InGaN/GaN multi-quantum wells. High crystal quality structures such as the nano-cone, nanopillar array and single pillar were fabricated based on the FIB method. During the fabrication process, various approaches were designed to minimize FIB damage caused by Gallium ion bombardment. The fabrication process for nano-cone is a combination of mask preparation by FIB with subsequent reactive ion etching (RIE). For fabricating nanopillar arrays, the nanopillars were patterned directly using FIB with an optimized beam current followed by wet etching process to remove the damage. On the other hand, the single pillar is achieved by gradually decreasing the ion beam current as the diameter of the pillar becomes smaller. The first order Raman spectra for the nanopillar array reveal a strong additional peak when the diameter of the nanopillars is less than 220 nm. This peak can also be observed in GaN pillars without MQW and is clearly assigned to the surface optical (SO) mode originated from the A1 phonon in wurtzite GaN. The frequency of this SO mode is found to be sensitive with the diameter and surface roughness of the nanopillars. Temperature-variable photoluminescence (PL) measurements show that a broadband emission in the as-grown sample split into the two well-resolved bands for nanopillars and the emission band at the higher energy side quickly thermally quenched. Room temperature PL measurements on the single pillars exhibit an increasing blue-shift of the peak emission with the decreasing of the pillar diameter. Additional simulation data and excitation power dependent PL studies confirm the observation of strain relaxation in the pillar’s MQW due to FIB fabrication. The temperature variable PL on the single pillar shows a monotonous blue shift as the temperature arises to 300 K. / published_or_final_version / Electrical and Electronic Engineering / Master / Master of Philosophy

The observation of graphene’s extraordinary electrical properties has stirred great interest in two dimensional (2D) materials. The rapid pace of discovery for low dimensional materials with exciting properties continue with graphene allotropes, multiple polymorphs of borophene, germanene, and many others. The future of 2D materials goes beyond synthesis and characterization of free standing materials and on to the construction of heterostructures or sophisticated multilayer devices. Knowledge about the resulting local structure and composition of such systems will be key to understanding and optimizing their performance characteristics. 2D materials do not have a repeating crystal structure which can be easily characterized using bulk methods and therefore a localized high resolution method is needed. Electron microscopy is well suited for characterizing 2D materials as a repeating coherent structure is not necessary to produce a measureable signal as may be the case for diffraction methods. A unique opportunity for fine local scale measurements in low dimensional systems exists with a specific class of materials known as ferecrystals, the rotationally disordered relative of misfit layer compounds. Ferecrystals provide an excellent test system to observe effects at heterostructure interfaces as the whole film is composed of interdigitated two dimensional layers. Therefore bulk methods can be used to corroborate local scale measurements. From the qualitative interpretation of high resolution scanning transmission electron microscope (STEM) images to the quantitative application of STEM energy dispersive X-ray spectroscopy (EDX), this thesis uses numerous methods electron microscopy. The culmination of this work is seen at the end of the thesis where atomically resolved STEM-EDX hyperspectral maps could be used to measure element specific atomic distances and the atomically resolved fractional occupancies of a low dimensional alloy. These local scale measurements are corroborated by additional experimental data. The input of multiple techniques leads to improved certainty in local scale measurements and the applicability of these methods to non-ferecrystal low dimensional systems.

O campo da modificação de materiais, através da implantação iônica, vem crescendo amplamente, impulsionado pelas aplicações tecnológicas na biologia, medicina, eletrônica, e outras áreas. Um dos aspectos relacionados ao entendimento desses novos materiais é a identificação e caracterização dos danos produzidos, após a irradiação. Nesse trabalho, foi proposto estudar as modificações microscópicas, após irradiação com feixe de íons de alta energia, em três diferentes polímeros: o policarbonato(Makrofol KG), com espessura de 8 &#181;m; o polialil diglicol carbonato PADC (CR39), espessura 900 &#181;m; e o nitrato de celulose (LR115), espessura 12&#181;m. As amostras foram irradiadas com feixe de Au de 350 MeV no acelerador Cíclotron do Hahn-Meitner Institut (HMI) em Berlim. As amostras de Makrofol KG foram dispostas em superposição de 6 folhas posicionadas perpendicularmente à direção do feixe e foram irradiadas com fluências de 10^8, 10^9 e 10^11 íons/cm^2. As amostras de CR39 e LR115 foram irradiadas com fluência de 10^9 íons/cm^2, sem superposição das amostras. O estudo comparativo dos danos estruturais nas amostras, antes e após a irradiação, foi realizado através de técnicas analíticas como Espectroscopia de Absorção no Infravermelho por Transformada de Fourier (FTIR), Difração de Raios X (XRD), Análise com Detecção de Recuo Elástico (ERDA), e Corrosão Química, para visualização e caracterização dos poros através do microscópio óptico e microscópio eletrônico de varredura. A análise FTIR das amostras mostrou haver diminuição do número de ligações simples, em favor do aumento do número de ligações duplas e triplas, após irradiação das amostras. Além disso, observou-se que a intensidade dos danos observados aumenta com o poder de freamento médio dos íons de Au durante a penetração nas amostras. A análise XRD, por sua vez, permitiu verificar um decréscimo da cristalinidade do Makrofol KG irradiado, enquanto observou-se indicações de variação da densidade do CR39, após irradiação, e inexistência de variação no LR115. A metodologia proposta para análise das amostras através da técnica ERDA não se mostrou eficiente para determinar a variação no teor de H das mesmas após a irradiação, não sendo possível obter resultados conclusivos para as amostras. Na análise dos poros, após corrosão química, observou-se diferentes comportamentos. As amostras de CR39 apresentaram uma evolução de superfície porosa para superfície pontiaguda com o aumento do tempo de corrosão, e obteve-se o valor Va = 1,213 (17) &#181;m/h para a velocidade de abertura do poros. Por outro lado, as diferentes folhas de Makrofol KG mantiveram a topografia porosa, sendo que a velocidade de abertura dos poros apresentou dependência com o poder de freamento dos íons na irradiação. Comparando amostras com valores semelhantes do poder de freamento, o resultado de Va obtido para o Makrofol é cerca de três vezes maior que o obtido para o CR39. / The research in the field of material modification with ion implantation has greately improved, stimulated by technological applications in biology, medicine, electronics and other related areas. One of the correlated aspects in understanding these new materials is the identification and characterization of the damage produced by ion beam irradiation. In this work, we propose to identify the microscopic modification in polymers, after their irradiation with a high energy beam. Three polymers have been used: polycarbonate foils (Makrofol KG), 8 &#181;m thick; polyalyl diglycol carbonate PADC (CR39) 900 &#181;m thick and cellulose nitrate(LR115) 12 &#181;m thick. The samples were irradiated with 350 MeV Au beam from the Cyclotron accelerator at Hahn-Meitner Institut (HMI) in Berlin. The Makrofol samples were placed in a 6-foil stack positioned in normal direction relative to the incident beam, in order to stop the projectiles. The irradiations were performed with ion fluences of 10^8, 10^9 e 10^11 ions/cm^2. The CR39 and LR115 samples, thicker than the range, were irradiated with the fluency of 10^9 ions/cm^2. The investigation of structural damage in the samples, after irradiation, was performed through analytical techniques such as: Fourier Transform Infrared Absorption Spectroscopy (FTIR), X Ray Difraction (XRD), Elastic Recoil Detection Analysis (ERDA), and Etching, followed by pore characterization using an optical and a scanning electron microscopes. The FTIR analysis of the samples showed a decrease in the number of simple bonds and an increase in the number of double and triple bonds, after irradiation. Moreover, it was observed that the damage intensity increases with the mean stopping power of Au. The XRD analysis allowed the observation of crystallinity decrease in Makrofol, and gave indications about a possible deviation in CR39 density, after sample irradiation, and no variation in LR115 samples. The methodology proposed using ERDA technique was not eficient to determine the H atoms teor in the polymers after irradiation, so, it was not possible to get conclusive results from the data. In the pore analysis, after etching, different behaviors were observed. The CR39 samples showed an evolution from a porous surface to a sharply peaked surface and a pore opening rate Va = 1,213 (17) &#181;m/h was obtained. On the contrary, different Makrofol KG foils preserved the porous topography for different etching times. The pore opening rate showed dependence with ion stopping power in the irradiation. Comparing samples with similar values of stopping power, the result is that Makrofol Va is three times greater than the obtained to CR39.